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GB1558553A - Calcium-selective electrode - Google Patents

Calcium-selective electrode Download PDF

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Publication number
GB1558553A
GB1558553A GB1117278A GB1117278A GB1558553A GB 1558553 A GB1558553 A GB 1558553A GB 1117278 A GB1117278 A GB 1117278A GB 1117278 A GB1117278 A GB 1117278A GB 1558553 A GB1558553 A GB 1558553A
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GB
United Kingdom
Prior art keywords
electrode
selective
electrode according
calcium
tube
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Expired
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GB1117278A
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NAT RES DEV
National Research Development Corp of India
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NAT RES DEV
National Research Development Corp of India
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Publication date
Application filed by NAT RES DEV, National Research Development Corp of India filed Critical NAT RES DEV
Priority to GB1117278A priority Critical patent/GB1558553A/en
Publication of GB1558553A publication Critical patent/GB1558553A/en
Expired legal-status Critical Current

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    • GPHYSICS
    • G01MEASURING; TESTING
    • G01NINVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
    • G01N27/00Investigating or analysing materials by the use of electric, electrochemical, or magnetic means
    • G01N27/26Investigating or analysing materials by the use of electric, electrochemical, or magnetic means by investigating electrochemical variables; by using electrolysis or electrophoresis
    • G01N27/28Electrolytic cell components
    • G01N27/30Electrodes, e.g. test electrodes; Half-cells
    • G01N27/333Ion-selective electrodes or membranes
    • G01N27/3335Ion-selective electrodes or membranes the membrane containing at least one organic component

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  • Chemical & Material Sciences (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Health & Medical Sciences (AREA)
  • Physics & Mathematics (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • Molecular Biology (AREA)
  • Analytical Chemistry (AREA)
  • Biochemistry (AREA)
  • General Health & Medical Sciences (AREA)
  • General Physics & Mathematics (AREA)
  • Immunology (AREA)
  • Pathology (AREA)
  • Electrolytic Production Of Non-Metals, Compounds, Apparatuses Therefor (AREA)

Description

(54) CALCIUM-SELECTIVE ELECTRODE (71) We, NATIONAL RESEARCH DEVELOPMENT CORPORATION, a British corporation established by statute, of Kingsgate House, 66-74 Victoria Street, London S.W.1., do hereby declare the invention for which we pray that a patent may be granted to us, and the method by which it is to be performed, to be particularly described in and by the following state ment:- This invention relates to a calciumselective electrode, and includes a method of making it and extends to the use of it.
According to the invention, a calciumselective electrode has an electrically conductive member in contact with an ionselective membrane (preferably from 0.01 to 0.3mm thick) comprising the cyclosilox maize compound ((CH;)2SiO)l2, of which up to one CH3 group on each silicon may be substituted. The electrically conductive member may be of platinum. and is preferably in the form of a sheet. The sheet may close one end of a non-conductive tube thrpugh which passes a wire electrically contacting the sheet. Optionally, a conductive screen may surround the tube (but not the sheet), and the electrode may further comprise an outer non-conductive tube surrounding the screen, such that the exterior surface of the electrode presents only said outer tube and said ion-selective membrane.
The ion-selective membrane preferably also comprises a film-forming polymer such as polyvinylchloride, which may account for 10% to 50% (e.g. 30%) by weight of the ion-selective membrane. The ion-selective membrane may be formed by applying to the (preferably abraded) sheet a solution (in a volatile solvent (e.g. cyclohexanone)) of the cyclosiloxane compound and of any film-forming polymer. The solvent may account for 70% to 95% by volume of the solution.
The cyclosiloxane compound may be made as described in UK Patent Specification 1162075, the resulting mixture of siloxanes being separated from the desired twelve-member cyclosiloxane compound by any desired method. Up to one methyl group on each silicon can be substituted, for example being ethyl, chloroethyl, propyl or viny. Conventional methods include molecular sieve techniques and gas chromatography, but the most successful method appears to be gel chromatography.
The invention will now be described by way of example with reference to the accompanying drawing, which shows schematically a sectional elevation of an electrode according to the invention.
Using the method described in UK Patent No. 1162075, a mixture of cyclosiloxanes was obtained. The mixture was separated using tetrahydrofuran as solvent and a gel permeation material of molecular weight exclusion limit of 1400. This material is a dry powder commercially available as Bio-beads SX2 consisting of styrene/divinylbenzene copolymer beads which are pre-swollen for 4 hours with tetrahydrofuran to form a homogeneous gel, and rinsed for 8 hours with tetrahydrofuran. A solution of 5g of siloxane mixture in 10ml of tetrahydrofuran was run into the top of a column 2.5m high by 50mm diameter of the Bio-beads, eluted with tetrahydrofuran at the rate of 100 ml/hour. and after about 1 - 2 hours the separated cyclosiloxanes emerged.The desired twelve-membered cyclosiloxane compound ((CH3)2SiO)12 was isolated in a yield as high as 15%, which exceeds the yield obtained by gas chromatography, fractional distillation and other techniques, and is believed to be 95% of all the twelvemembered compound in the cyclosiloxane mixture. The cyclosiloxane is now put aside.
A copper wire 2, for attachment at its upper (free) end to desired electrical apparatus. is soldered in contact with a platinum sheet in the form of a plate 4 (through an intermediate platinum wire 2a). The plate 4 is lmm thick and Smm in diameter, and closes the lower end of a glass tube 6 through which the wire 2 passes.
For protection from interference, the tube 6 is surrounded by a copper screen 8, which itself is surrounded by an outer glass tube 10. The tubes 6 and 10 are sealed together at the bottom. The screen 8 is held in position by an annular filler 12 of an epoxy resin. The plate 4 is heat-sealed into the glass.
At the upper end of the outer tube 10, a similar resin 14 holds the screen 8 and inner tube 6. The screen 8 is electrically connected by turns of wire 15 to the screening of a coaxial-screened cable 16, and the wire 2 is soldered at 18 to the central conductor of the cable 16. Insulation and rigidity are assured by potting with an epoxy resin 20, the whole assembly at the upper end of the outer tube 10 being protected by a rubber cap 22.
Returning to the lower end of the outer tube 10, all that is presented externally is the glass tube 10 and the plate 4. To render this calcium-selective, the plate 4 and surrounding glass are lightly abraded with emery paper and dipped in a solution consisting of 90 parts (by weight) of cyclohexanone. 3 parts of polyvinylchloride and 7 parts of the cyclosiloxane ((CH3)2SiO)l2 prepared as described earlier. Upon being allowed to dry, an ion-selective layer in the form of a membrane 24 which may be 0.01 to 0.3mm thick forms an intimate contact with the platinum plate 4. This membrane is allowed to dry out thoroughly, for 24 hours, and is then conditioned, to make it ready for use, by holding for 24 hours in a centimolar aqueous solution of calcium chloride.
The resulting assembly forms a robust calcium-selective electrode with mechanically sound membrane/platinum contact.
Over a range of conditions. the electrode is highly selective towards calcium. whose concentration it can with reasonable accuracy monitor throughout the range 10 to 10-5M, with a response linear to log (CaT: concentration) in the range 4 x 10-2M to S x 10-5M. The response time depends on concentration and on any interfering ions present, but is generally less than 10 seconds.
The electrode remains selective towards calcium down to pH 1.6. From pH 1.6 to 4.5, response is independent of pH. From 4.5 to 12 there is a pH-dependent decrease in response but, at any given pH up to 9.
response to Ca+ ions is Nernstian.
WHAT WE CLAIM IS: 1. A calcium-selective electrode having an electrically conductive member in contact with an ion-selective membrane comprising the cyclosiloxane compound ((CH3)2SiO)l2 of which up to one CH3 group on each silicon may be substituted.
2. An electrode according to claim 1, wherein the electrically conductive member is of platinum.
3. An electrode according to claim 1 or 2, wherein the electrically conductive member is in the form of a sheet.
4. An electrode according to claim 3, further comprising a non-conductive tube closed at one end by the sheet, through which tube there passes a wire electrically contacting the sheet.
5. An electrode according to claim 4, further comprising a conductive screen surrounding the tube.
6. An electrode according to claim 5, further comprising a non-conductive outer tube surrounding the screen, such that the exterior surfaces of the electrode presents only said outer tube and said ion-selective membrane.
7. An electrode according to any preceding claim, wherein the ion-selective membrane has a thickness of up to 0.3mm.
8. An electrode according to any preceding claim, wherein the ion-selective membrane has a thickness of at least O.Olmm.
9. An electrode according to any preceding claim, wherein the ion-selective membrane also comprises a film-forming polymer.
10. An electrode according to claim 9, wherein the film-forming polymer accounts for 10 to 50% by weight of the ion-selective membrane.
11. A calcium-selective electrode substantially as hereinbefore described with reference to and as shown in the accompanying drawing.
12. A method of making an electrode according to any preceding claim, comprises ing dipping the electrically conductive member in a solution containing the said cyclosiloxane compound, and allowing the dipped member to drv.
13. A method according to claim 12, wherein the solution comprises from 70 to 95% by weight of a solvent for the cyclosilo xane compound.
14. A method according to claim 13, wherein the solvent is cyclohexanone.
15. A method according to claim 12. 13 or 14. wherein the solution further contains a film-forming polymer.
16. A method of making an electrode according to any of claims 1 to 11, wherein said cyclosiloxane compound was isolated from a mixture of cvclosiloxane compounds by gel chromatography.
17. A method of making an electrode according to any of claims 1 to 11, the method being substantially as hereinbefore described.
**WARNING** end of DESC field may overlap start of CLMS **.

Claims (19)

**WARNING** start of CLMS field may overlap end of DESC **. sheet in the form of a plate 4 (through an intermediate platinum wire 2a). The plate 4 is lmm thick and Smm in diameter, and closes the lower end of a glass tube 6 through which the wire 2 passes. For protection from interference, the tube 6 is surrounded by a copper screen 8, which itself is surrounded by an outer glass tube 10. The tubes 6 and 10 are sealed together at the bottom. The screen 8 is held in position by an annular filler 12 of an epoxy resin. The plate 4 is heat-sealed into the glass. At the upper end of the outer tube 10, a similar resin 14 holds the screen 8 and inner tube 6. The screen 8 is electrically connected by turns of wire 15 to the screening of a coaxial-screened cable 16, and the wire 2 is soldered at 18 to the central conductor of the cable 16. Insulation and rigidity are assured by potting with an epoxy resin 20, the whole assembly at the upper end of the outer tube 10 being protected by a rubber cap 22. Returning to the lower end of the outer tube 10, all that is presented externally is the glass tube 10 and the plate 4. To render this calcium-selective, the plate 4 and surrounding glass are lightly abraded with emery paper and dipped in a solution consisting of 90 parts (by weight) of cyclohexanone. 3 parts of polyvinylchloride and 7 parts of the cyclosiloxane ((CH3)2SiO)l2 prepared as described earlier. Upon being allowed to dry, an ion-selective layer in the form of a membrane 24 which may be 0.01 to 0.3mm thick forms an intimate contact with the platinum plate 4. This membrane is allowed to dry out thoroughly, for 24 hours, and is then conditioned, to make it ready for use, by holding for 24 hours in a centimolar aqueous solution of calcium chloride. The resulting assembly forms a robust calcium-selective electrode with mechanically sound membrane/platinum contact. Over a range of conditions. the electrode is highly selective towards calcium. whose concentration it can with reasonable accuracy monitor throughout the range 10 to 10-5M, with a response linear to log (CaT: concentration) in the range 4 x 10-2M to S x 10-5M. The response time depends on concentration and on any interfering ions present, but is generally less than 10 seconds. The electrode remains selective towards calcium down to pH 1.6. From pH 1.6 to 4.5, response is independent of pH. From 4.5 to 12 there is a pH-dependent decrease in response but, at any given pH up to 9. response to Ca+ ions is Nernstian. WHAT WE CLAIM IS:
1. A calcium-selective electrode having an electrically conductive member in contact with an ion-selective membrane comprising the cyclosiloxane compound ((CH3)2SiO)l2 of which up to one CH3 group on each silicon may be substituted.
2. An electrode according to claim 1, wherein the electrically conductive member is of platinum.
3. An electrode according to claim 1 or 2, wherein the electrically conductive member is in the form of a sheet.
4. An electrode according to claim 3, further comprising a non-conductive tube closed at one end by the sheet, through which tube there passes a wire electrically contacting the sheet.
5. An electrode according to claim 4, further comprising a conductive screen surrounding the tube.
6. An electrode according to claim 5, further comprising a non-conductive outer tube surrounding the screen, such that the exterior surfaces of the electrode presents only said outer tube and said ion-selective membrane.
7. An electrode according to any preceding claim, wherein the ion-selective membrane has a thickness of up to 0.3mm.
8. An electrode according to any preceding claim, wherein the ion-selective membrane has a thickness of at least O.Olmm.
9. An electrode according to any preceding claim, wherein the ion-selective membrane also comprises a film-forming polymer.
10. An electrode according to claim 9, wherein the film-forming polymer accounts for 10 to 50% by weight of the ion-selective membrane.
11. A calcium-selective electrode substantially as hereinbefore described with reference to and as shown in the accompanying drawing.
12. A method of making an electrode according to any preceding claim, comprises ing dipping the electrically conductive member in a solution containing the said cyclosiloxane compound, and allowing the dipped member to drv.
13. A method according to claim 12, wherein the solution comprises from 70 to 95% by weight of a solvent for the cyclosilo xane compound.
14. A method according to claim 13, wherein the solvent is cyclohexanone.
15. A method according to claim 12. 13 or 14. wherein the solution further contains a film-forming polymer.
16. A method of making an electrode according to any of claims 1 to 11, wherein said cyclosiloxane compound was isolated from a mixture of cvclosiloxane compounds by gel chromatography.
17. A method of making an electrode according to any of claims 1 to 11, the method being substantially as hereinbefore described.
18. A calcium-selective electrode made
by a method according to any of claims 12 to 17.
19. A method of determining calcium in a solution, comprising using an electrode according to any of claims 1 to 11 or 18.
GB1117278A 1978-03-21 1978-03-21 Calcium-selective electrode Expired GB1558553A (en)

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Application Number Priority Date Filing Date Title
GB1117278A GB1558553A (en) 1978-03-21 1978-03-21 Calcium-selective electrode

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Application Number Priority Date Filing Date Title
GB1117278A GB1558553A (en) 1978-03-21 1978-03-21 Calcium-selective electrode

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Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4388165A (en) * 1981-02-28 1983-06-14 Olympus Optical Company Ltd. Selective ion sensitive electrode and method of making it
US4388167A (en) * 1981-09-07 1983-06-14 Olympus Optical Company Limited Ion selective electrode
DE3230147A1 (en) * 1982-08-13 1984-02-16 Licentia Patent-Verwaltungs-Gmbh, 6000 Frankfurt Ion-sensitive layer
EP0157434A1 (en) * 1984-02-29 1985-10-09 Nihon Parkerizing Co., Ltd. Process for regulating the zinc and/or nickel content in phosphatizing solutions

Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4388165A (en) * 1981-02-28 1983-06-14 Olympus Optical Company Ltd. Selective ion sensitive electrode and method of making it
US4388167A (en) * 1981-09-07 1983-06-14 Olympus Optical Company Limited Ion selective electrode
DE3230147A1 (en) * 1982-08-13 1984-02-16 Licentia Patent-Verwaltungs-Gmbh, 6000 Frankfurt Ion-sensitive layer
EP0157434A1 (en) * 1984-02-29 1985-10-09 Nihon Parkerizing Co., Ltd. Process for regulating the zinc and/or nickel content in phosphatizing solutions

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